Bioinspired Mechanical Gradients in Cellulose Nanofibril/Polymer Nanopapers

Wang, Baochun; Benítez, Alejandro J.; Lossada, Francisco; Merindol, Rémi; Walther, Andreas

doi:10.1002/anie.201511512

Cited by 62 publications

(45 citation statements)

References 51 publications

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“…A mechanical gradient is often obtained by varying the structures or components along an axis of materials, including filler content, degree of orientation, and crosslinking density . Here, we introduced mechanical gradients by varying Cu‐DOU hard phase content.…”

Section: Resultsmentioning

confidence: 99%

Biomimetic Materials with Multiple Protective Functionalities

Liu

Zhang

Guan

et al. 2019

Adv Funct Materials

111

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Natural tissues possess superior material properties such as self-healing, mechanical robustness, and mechanical gradients that allow organisms to adapt and survive in dangerous environments. Although highly desired, imparting synthetic materials with these biomimetic protective features remains a challenge. Here, the versatile dimethylglyoxime-urethane (DOU) moiety is used to create a multifunctional polyurethane (DOU-PU). The reactivities of DOU including reversible dissociation, metal coordination, photolysis enabled self-healing, high strength and toughness, mechanical gradient formation, and spatially controlled functionalization. By incorporating DOU, a multifunctional protective film is produced with superior resistance to mechanical damage, rapid room temperature self-healing, and anti-counterfeiting features. This super biomimetic film is expected to be very useful for the protection of various types of valuable objects such as electronics, diplomas, currency, and automobiles.

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Section: Resultsmentioning

confidence: 99%

Biomimetic Materials with Multiple Protective Functionalities

Liu

Zhang

Guan

et al. 2019

Adv Funct Materials

111

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“…Additionally, they can form tight cohesion with cellulose in the bulk phase by hydrogen bonding. 29,30 We denote these copolymers as EG x DMAm y , whereby the subscripts denote the molar fractions in the final material as determined by 1 H NMR. The resulting copolymers were characterized by gel 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60 permeation chromatography (GPC), 1 H NMR, and differential scanning calorimetry (DSC; Table 1, Figures 1a-c and S1).…”

Section: Resultsmentioning

confidence: 99%

Understanding Toughness in Bioinspired Cellulose Nanofibril/Polymer Nanocomposites

et al. 2016

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Cellulose nanofibrils (CNFs) are considered next generation, renewable reinforcements for sustainable, high-performance bioinspired nanocomposites uniting high stiffness, strength and toughness. However, the challenges associated with making well-defined CNF/polymer nanopaper hybrid structures with well-controlled polymer properties have so far hampered to deduce a quantitative picture of the mechanical properties space and deformation mechanisms, and limits the ability to tune and control the mechanical properties by rational design criteria. Here, we discuss detailed insights on how the thermo-mechanical properties of tailor-made copolymers govern the tensile properties in bioinspired CNF/polymer settings, hence at high fractions of reinforcements and under nanoconfinement conditions for the polymers. To this end, we synthesize a series of fully water-soluble and nonionic copolymers, whose glass transition temperatures (Tg) are varied from -60 to 130 °C. We demonstrate that well-defined polymer-coated core/shell nanofibrils form at intermediate stages and that well-defined nanopaper structures with tunable nanostructure arise. The systematic correlation between the thermal transitions in the (co)polymers, as well as its fraction, on the mechanical properties and deformation mechanisms of the nanocomposites is underscored by tensile tests, SEM imaging of fracture surfaces and dynamic mechanical analysis. An optimum toughness is obtained for copolymers with a Tg close to the testing temperature, where the soft phase possesses the best combination of high molecular mobility and cohesive strength. New deformation modes are activated for the toughest compositions. Our study establishes quantitative structure/property relationships in CNF/(co)polymer nanopapers and opens the design space for future, rational molecular engineering using reversible supramolecular bonds or covalent cross-linking.

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“…The shear‐induced alignment of anisotropic building blocks, including carbon fibers, silicon carbide whiskers, alumina platelets, and nanofibrillated cellulose (NFC) during direct ink writing enables the fabrication of textured 3D structured composites with enhanced mechanical properties and other functionalities. For cellulose‐based materials, efforts to date have focused primarily on hydrogel‐based inks that contain low NFC loading (0.8–2.5 wt%) . While the inherently entangled state of concentrated NFC suspensions prevent high loading, less concentrated NFC‐filled inks typically require thickening agents, such as fumed silica, laponite, or high molecular weight polymers, to achieve the desired rheological properties for direct ink writing.…”

Section: Introductionmentioning

confidence: 99%

Cellulose Nanocrystal Inks for 3D Printing of Textured Cellular Architectures

Siqueira

Kokkinis

Libanori

et al. 2017

Adv Funct Materials

513

434

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3D printing of renewable building blocks like cellulose nanocrystals offers an attractive pathway for fabricating sustainable structures. Here, viscoelastic inks composed of anisotropic cellulose nanocrystals (CNC) that enable patterning of 3D objects by direct ink writing are designed and formulated. These concentrated inks are composed of CNC particles suspended in either water or a photopolymerizable monomer solution. The shear-induced alignment of these anisotropic building blocks during printing is quantified by atomic force microscopy, polarized light microscopy, and 2D wide-angle X-ray scattering measurements. Akin to the microreinforcing effect in plant cell walls, the alignment of CNC particles during direct writing yields textured composites with enhanced stiffness along the printing direction. The observations serve as an important step forward toward the development of sustainable materials for 3D printing of cellular architectures with tailored mechanical properties.

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Bioinspired Mechanical Gradients in Cellulose Nanofibril/Polymer Nanopapers

Cited by 62 publications

References 51 publications

Biomimetic Materials with Multiple Protective Functionalities

Biomimetic Materials with Multiple Protective Functionalities

Understanding Toughness in Bioinspired Cellulose Nanofibril/Polymer Nanocomposites

Cellulose Nanocrystal Inks for 3D Printing of Textured Cellular Architectures

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